Platinum Single-Atom Nests Boost Solar-Driven Photocatalytic Non-Oxidative Coupling of Methane to Ethane - Details

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This　work　introduces　a　new　strategy　of　a　single-atom　nest　catalyst,　whereby　several　single　atoms　are　positioned　closely,　aiming　to　achieve　the　dual　benefits　of　high　atom-utilization　efficiency　while　avoiding　the　steric　hindrance　in　the　coupling　reaction.　As　a　proof　of　concept,　Pt　single-atom　nests,　where　the　adjacent　Pt　single　atoms　are　approximately　4　Å　apart,　are　precisely　engineered　on　the　TiO2　photocatalyst　for　photocatalytic　non-oxidative　coupling　of　methane.　The　Pt　single-atom　nest　photocatalyst　demonstrates　remarkable　activity,　achieving　a　C2H6　yield　and　turnover　frequency　of　251.6　μmol　gcat-1　h-1　and　20　h-1,　respectively,　representing　a　3.2-fold　improvement　compared　to　the　Pt　single-atom　photocatalyst.　Density　functional　theory　calculations　reveal　that　the　Pt　single-atom　nest　can　significantly　decrease　the　energy　barrier　for　the　activation　of　both　CH4　molecules　in　the　coupling　process.　©　2024　American　Chemical　Society.

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[ 1 ] [Zhang P.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 2 ] [Zhang P.]Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes, Ministry of Education, College of Environment, Hohai University, Nanjing, 210098, China
[ 3 ] [Li J.]Department of Chemical Engineering, KU Leuven, Celestijnenlaan 200F, Leuven, 3001, Belgium
[ 4 ] [Huang H.]School of Energy and Environment, Southeast University, Nanjing, 210096, China
[ 5 ] [Sui X.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 6 ] [Zeng H.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 7 ] [Lu H.]Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensl, St Lucia, 4072, QLD, Australia
[ 8 ] [Wang Y.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 9 ] [Jia Y.]Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, China
[ 10 ] [Steele J.A.]Australian Institute for Bioengineering and Nanotechnology and School of Mathematics and Physics, The University of Queensl, Brisbane, 4072, QLD, Australia
[ 11 ] [Ao Y.]Key Laboratory of Integrated Regulation and Resource Development on Shallow Lakes, Ministry of Education, College of Environment, Hohai University, Nanjing, 210098, China
[ 12 ] [Roeffaers M.B.J.]Centre for Membrane Separations, Adsorption, Catalysis and Spectroscopy for Sustainable Solutions (cMACS), KU Leuven, Celestijnenlaan 200F, Leuven, B-3001, Belgium
[ 13 ] [Dai S.]Key Laboratory for Advanced Materials and Feringa Nobel Prize Scientist Joint Research Center, Institute of Fine Chemicals, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, China
[ 14 ] [Zhang Z.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 15 ] [Wang L.]Nanomaterials Centre, School of Chemical Engineering, Australian Institute for Bioengineering and Nanotechnology, The University of Queensl, St Lucia, 4072, QLD, Australia
[ 16 ] [Fu X.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China
[ 17 ] [Long J.]State Key Lab of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China

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Journal of the American Chemical Society

ISSN： 0002-7863

Year： 2024

Issue： 34

Volume： 146

Page： 24150-24157

1 4 . 5 0 0

JCR@2023

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SCOPUS Cited Count： 11

ESI Highly Cited Papers on the List： 0 Unfold All

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30 Days PV： 2

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